Well let's see, many tend to be Ax Crazy (making them anywhere from Neutral Evil to Chaotic Evil), and if they're on the good guys' team, they might be the Token Evil Teammate as well as Type V Anti-Hero (which often overlaps with Villain Protagonist due to the Type V Anti-Hero having no motively good intentions), and very rarely is one ever of a genuinely good alignment due to their Ax Crazy tendencies, making them Chaotic Neutral at best and Chaotic Evil at worst.

They would be more 'chaotic neutral'. After all, what's to say about them? They're basically mentally unstable but initially caring and protective.

Take Yuno Gasai for example.

Yuno's of the Chaotic Evil Type I into IV variety. Not to mention, many are ax crazy, placing most of them into the chaotic evil alingment, and if they're on the good guy team, they're often the token evil teammate as well as type v anti hero. They're rarely of a good alignment due to their ax crazy tendencies.

@AnimeKami: Yuno's a villain, and also an expy that's basically the most repulsive parts of Johann Liebert from Monster and Lucy from Elfen Lied reconstituted into one humanoid mass, combining the depravity from Johann and the insanity and hair & eye color of Lucy. Doesn't help that they're the more savage variety of Yanderes.

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